Permeable Proton Transport and Hydrogenation Attained by ONCS-Induced Graphene Nanosheet Film for Neuromorphic Memory...

Traditional von Neumann architecture-based devices are limited by the memory wall, hindering the development of next-generation artificial intelligence. Controlling proton transport to achieve hydrogenation in monolayer graphene resulting in the reversible and controllable nature of their memristive behavior has attracted significant interest for neuromorphic applications. However, multilayer graphene is impermeable to protons and most ions, which severely restricts the development of graphene-based neuromorphic devices in practice. To address this challenge, we developed a three-terminal artificial synapse based on stacked graphene nanosheets induced by an organic nano carbon source (ONCS). The device achieves co-regulated proton transport and hydrogenation through the gate-source voltage (V_GS) and source-drain voltage (V_DS), enabling dual-stimulus memristive effects (gate stimulus and source-drain stimulus). It successfully mimics essential synaptic functions, including short-term depression (STD), long-term depression (LTD), and paired-pulse depression (PPD) with intensity-dependent and pulse number-sensitive responses. This work resolves the ion-electron co-regulation challenge in multilayer graphene for next-generation AI computing.